Abstract
An overview is given of the molecular quantum electrodynamical (QED) theory of resonance energy transfer (RET). In this quantized radiation field description, RET arises from the exchange of a single virtual photon between excited donor and unexcited acceptor species. Diagrammatic time-dependent perturbation theory is employed to calculate the transfer matrix element, from which the migration rate is obtained via the Fermi golden rule. Rate formulae for oriented and isotropic systems hold for all pair separation distances, R, beyond wave function overlap. The two well-known mechanisms associated with migration of energy, namely the R−6 radiationless transfer rate due to Förster and the R−2 radiative exchange, correspond to near- and far-zone asymptotes of the general result. Discriminatory pair transfer rates are also presented. The influence of an environment is accounted for by invoking the polariton, which mediates exchange and by introducing a complex refractive index to describe local field and screening effects. This macroscopic treatment is compared and contrasted with a microscopic analysis in which the role of a neutral, polarizable and passive third-particle in mediating transfer of energy is considered. Three possible coupling mechanisms arise, each requiring summation over 24 time-ordered diagrams at fourth-order of perturbation theory with the total rate being a sum of two- and various three-body terms.
Highlights
A wide-ranging fundamental process is the transfer of energy between matter [1]
The intrinsic importance of the problem of resonance energy transfer (RET) is evident from its formulation, as stated above and the fact that it manifests in an inordinately large number of varied scientific and engineering situations and applications ranging from revealing structural information on biomolecules, to improving the functionality and efficiency of devices fabricated at the nanoscale [3,4,5,6,7,8,9]
Energy is relayed from donor to acceptor species via the exchange of a single virtual photon
Summary
A wide-ranging fundamental process is the transfer of energy between matter [1]. There are clearly spatio-temporal aspects that feature in the transfer process and which must be accounted for regardless of whether the exchange of energy is resonant or not since the donor and acceptor moieties are separated from one another in both the space and time dimensions. The intrinsic importance of the problem of resonance energy transfer (RET) is evident from its formulation, as stated above and the fact that it manifests in an inordinately large number of varied scientific and engineering situations and applications ranging from revealing structural information on biomolecules, to improving the functionality and efficiency of devices fabricated at the nanoscale [3,4,5,6,7,8,9]. (QED) to RET, concentrating first on the pair transfer rate before going on to examine the role of an additional microscopic particle or a medium on the exchange process
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